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Abstract Exsolution reactions enable the synthesis of oxide-supported metal nanoparticles, which are desirable as catalysts in green energy conversion technologies. It is crucial to precisely tailor the nanoparticle characteristics to optimize the catalysts’ functionality, and to maintain the catalytic performance under operation conditions. We use chemical (co)-doping to modify the defect chemistry of exsolution-active perovskite oxides and examine its influence on the mass transfer kinetics of Ni dopants towards the oxide surface and on the subsequent coalescence behavior of the exsolved nanoparticles during a continuous thermal reduction treatment. Nanoparticles that exsolve at the surface of the acceptor-type fast-oxygen-ion-conductor SrTi0.95Ni0.05O3−δ (STNi) show a high surface mobility leading to a very low thermal stability compared to nanoparticles that exsolve at the surface of donor-type SrTi0.9Nb0.05Ni0.05O3−δ (STNNi). Our analysis indicates that the low thermal stability of exsolved nanoparticles at the acceptor-doped perovskite surface is linked to a high oxygen vacancy concentration at the nanoparticle-oxide interface. For catalysts that require fast oxygen exchange kinetics, exsolution synthesis routes in dry hydrogen conditions may hence lead to accelerated degradation, while humid reaction conditions may mitigate this failure mechanism.

Highlights Vacancy in the transition metal layer of sodium cathode material induces the formation lone-pair electrons in the O 2p orbital. Material delivers more capacity from the oxygen redox validated by density functional calculation. Widened dominance of the OP4 phase without releasing O2 gas.

Abstract Solid–state batteries based on Li7La3Zr2O12 (LLZO) garnet electrolyte are a robust and safe alternative to conventional lithium‐ion batteries. However, the large‐scale implementation of ceramic composite cathodes is still challenging due to a complex multistep manufacturing process. A new one‐step route for the direct synthesis of LLZO during the manufacturing of LLZO/LiCoO2 (LCO) composite cathodes based on cheap precursors and utilizing the industrially established tape casting process is presented. It is shown that Al, Ta:LLZO can be formed directly in the presence of LCO from metal oxide precursors (LiOH, La2O3, ZrO2, Al2O3, and Ta2O5) by heating to 1050 °C, eliminating the time‐ and energy‐consuming synthesis of preformed LLZO powders. In addition, performance‐optimized gradient microstructures can be produced by sequential casting of slurries with different compositions, resulting in dense and flat phase‐pure cathodes without unwanted ion interdiffusion or secondary phase formation. Freestanding cathodes with a thickness of 85 µm, a relative density of 95%, and an industrial relevant LCO loading of 15 mg show an initial capacity of 82 mAh g−1 (63% of the theoretical capacity of LCO) in a solid‐state cell with Li metal anodes, which is comparable to conventional LCO/LLZO cathodes and can be further improved in the future.

Garnet-type solid electrolytes stand out as promising Li-ion conductors for the next-generation batteries. It has been demonstrated that the inherent properties of garnets can be tailored by introducing various dopants into their crystal structures. Recently, there has been a growing interest in the concept of high entropy stabilization for materials design. In this study, we synthesized high-entropy garnets denoted as Li6La3Zr0.7Ti0.3Ta0.5Sb0.5O12 (LLZTTSO), wherein Ti, Sb, and Ta occupy the Zr site. The formation of the cubic garnet phase in LLZTTSO was confirmed through X-ray diffraction (XRD), and the resulting lattice parameter agreed with predictions made using computational methods. Despite the substantial porosity (relative density 80.6%) attributed to the low sintering temperature, LLZTTSO exhibits a bulk ionic conductivity of 0.099 mS cm−1 at 25°C, and a total ionic conductivity of 0.088 mS cm−1, accompanied by an activation energy of 0.497 eV. Furthermore, LLZTTSO demonstrates a critical current density of 0.275 mA cm−2 at 25°C, showcasing its potential even without any interfacial modification.

This study explores multi-component garnet-based materials as solid electrolytes for all-solid-state lithium batteries. Through a combination of computational and experimental approaches, we investigate the thermodynamic and structural properties of lithium lanthanum zirconium oxide garnets doped with various elements. Applying density functional theory, the influence of dopants on the thermodynamic stability of these garnets was studied. Probable atomic configurations and their impact on materials’ properties were investigated with the focus on understanding the influence of these configurations on structural stability, phase preference, and ionic conductivity. In addition to the computational study, series of cubic-phase garnet compounds were synthesized and their electrochemical performance was evaluated experimentally. Our findings reveal that the stability of cubic phase in doped Li-garnets is primarily governed by enthalpy, with configurational entropy playing a secondary role. Moreover, we establish that the increased number of doping elements significantly enhances the cubic phase’s stability. This in-depth understanding of materials’ properties at atomic level establishes the basis for optimizing high-entropy ceramics, contributing significantly to the advancement of solid-state lithium batteries and other applications requiring innovative material solutions.

BaCe0.65Zr0.2Y0.15O3-δ (BCZ20Y15) has raised great interest due to its good protonic conductivity and chemical stability. However, the sintering of the material is considerably challenged by its refractory nature. In the current work, almost fully densified single-phase BCZ20Y15 with grain sizes exceeding 10 μm was successfully fabricated by sintering at 1500 °C by using calcined powders consisting of naturally separated perovskite phases and 0.5 wt% NiO. The role of NiO as sintering aid was elucidated by Inductively Coupled Plasma Optical Emission Spectroscopy (ICP-OES) and Atom Probe Tomography (APT) methods, concerning global and local material composition. Furthermore, the mechanism leading to the promoted densification and grain growth is elucidated based on current experimental results and a comprehensive review of the literature.

The increased interest in dual-phase membrane materials for oxygen separation leads to the continuous optimization of their composition. Rare-earth doped ceria is a promising candidate as the ion-conducting phase in the membrane. Spinel-structured FeCo2O4 was investigated as an electronic conducting phase forming an additional electronic conducting perovskite-structured phase during sintering when combined with Ce1−xLnxO2−δ. The influence of rare-earth lanthanide elements, i.e., Gd and Sm, as well as their concentration, i.e. x = 0.1 and 0.2, on the final phase composition and microstructure as well as its related functional properties in particular oxygen permeation is analyzed. 20 mol.% doping of either Gd or Sm reveals a multi-phase microstructure after sintering. Moreover, segregation of Gd/Sm, iron, and cobalt is found at the ceria-ceria grain boundaries in Ce0.8Sm0.2O2−δ- and Ce0.9Gd0.1O2−δ-based composites. In contrast, 10 mol.% Gd–doping leads to a dual-phase membrane material without the formation of any other phase. In all cases, the percolation threshold is reached at approx. 20 vol% of the electron-conducting phase in the system leading to similar maximum permeation rates determined by the ionic conductivity of the ceria phase.

Recycling of Nd–Fe–B magnets is an ongoing challenge regarding circular economy. State‐of‐the‐art magnet production methods, such as hot deformation, have limitations with respect to direct recycling of magnet scrap particles that differ from pristine melt‐spun Nd–Fe–B powder. Recent work has shown that a combination of presintering by field‐assisted sintering technology/spark plasma sintering (FAST/SPS) and hot deformation by flash spark plasma sintering (flash SPS) has the potential to directly produce Nd–Fe–B magnets from 100% scrap material. Both processes have the capability to adjust and monitor process parameters closely, resulting in recycled magnets with properties similar to commercial magnets but made directly from crushed and recycled Nd–Fe–B powder that partially or completely replaces pristine melt‐spun Nd–Fe–B powder. Herein, a systematic study is done inserting recycled magnet particles into a flash SPS deformed magnet, considering the effects of different weight percentages of scrap material of varied particle size fractions. In some cases, coercivity HcJ of >1400 kAm−1 and remanence Br of 1.1 T can be achieved with 20 wt% scrap material. The relationship between particle size fraction, oxygen uptake, and percentage of recyclate in a final magnet are all explored and discussed with respect to magnets made from pristine material.

Abstract The development of reliable and affordable all‐solid‐state sodium metal batteries (ASS‐SMBs) requires suitable solid‐state electrolytes with cost‐efficient processing and stabilized electrode/electrolyte interfaces. Here, an integrated porous/dense/porous Na5YSi4O12 (NYS) trilayered scaffold is designed and fabricated by tape casting using aqueous slurries. In this template‐based NYS scaffold, the dense layer in the middle serves as a separator and the porous layers on both sides accommodate the active materials with their volume changes during the charge/discharge processes, increasing the contact area and thus enhancing the utilization rate and homogenizing the current distribution. The Na/NYS/Na symmetric cells with the Pb‐coated NYS scaffold exhibit significantly reduced interfacial impedance and superior critical current density of up to 3.0 mA cm−2 against Na metal owing to enhanced wettability. Furthermore, the assembled Na/NYS/S full cells operated without external pressure at room temperature showed a high initial discharge capacity of 970 mAh g−1 and good cycling stability with a capacity of 600 mAh g−1 after 150 cycles (based on the mass of sulfur). This approach paves the way for the realization of economical and practical ASS‐SMBs from the perspective of ceramic manufacturing.

Developing cost-effective and reliable solid-state sodium batteries with superior performance is crucial for stationary energy storage. A key component in facilitating their application is a solid-state electrolyte with high conductivity and stability. Herein, we employed aliovalent cation substitution to enhance ionic conductivity while preserving the crystal structure. Optimized substitution of Y3+ with Zr4+ in Na5YSi4O12 introduced Na+ ​ion vacancies, resulting in high bulk and total conductivities of up to 6.5 and 3.3 ​mS ​cm−1, respectively, at room temperature with the composition Na4.92Y0.92Zr0.08Si4O12 (NYZS). NYZS shows exceptional electrochemical stability (up to 10 ​V vs. Na+/Na), favorable interfacial compatibility with Na, and an excellent critical current density of 2.4 ​mA ​cm−2. The enhanced conductivity of Na+ ​ions in NYZS was elucidated using solid-state nuclear magnetic resonance techniques and theoretical simulations, revealing two migration routes facilitated by the synergistic effect of increased Na+ ​ion vacancies and improved chemical environment due to Zr4+ substitution. NYZS extends the list of suitable solid-state electrolytes and enables the facile synthesis of stable, low-cost Na+ ion silicate electrolytes.

Battery solid-state electrolytes rely on mixed polyanion networks to attain high ionic conductivities. Here, the authors investigate the effect of polyanion mixing on the solid-state electrolyte ion conductivity via theoretical calculations and electrochemical measurements.

The increasing demand for safe energy storage has led to intensive investigations of solid-state Li+-ion conductors in the Li2O-M2O3–ZrO2–SiO2–P2O5 system. As a continuation of the cation substitution in this system, which we reported on very recently, a study of the impact of polyanionic substitutions on ionic conductivity was carried out here in two series, Li3+xSc2SixP3-xO12 (0 ≤ x ≤ 0.6) and Li1.2+xSc0.2Zr1.8SixP3-xO12 (0.3 ≤ x ≤ 2.8), with the aim of increasing ionic conductivity, determing the phase stability, and optimizing the processing conditions – especially decreasing the sintering temperatures – depending on the level of substitution.The polyanionic substitution, i.e. the substitution of (PO4)3- with (SiO4)4-, in the Li2O–Sc2O3–ZrO2–SiO2–P2O5 system revealed that a) the sintering temperature can effectively be reduced, b) the presence of zirconium can limit the evaporation of lithium species even at high sintering temperatures, c) the purity of the NaSICON materials has a strong influence on the grain boundary resistance, and therefore on the ionic conductivity, and d) the silicate substitution in Li3+xSc2SixP3-xO12 (0 ≤ x ≤ 0.6) stabilized the monoclinic polymorph (space group P21/n) with an enhanced total ionic conductivity at 25 °C from 6.5 × 10−7 S cm−1 to 1.2 × 10−5 S cm−1 for x = 0 to x = 0.15, respectively, exhibiting the highest ionic conductivity at 25 °C among the compositions investigated.

Abstract Advanced ceramic materials with tailored properties are at the core of established and emerging energy technologies. Applications encompass high‐temperature power generation, energy harvesting, and electrochemical conversion and storage. New opportunities for material design, the importance of processing and material integration, and the need for long‐term testing under realistic conditions are highlighted in the present perspective.

Dual-phase membranes are increasingly attracting attention as a solution for developing stable oxygen permeation membranes. Ce0.8Gd0.2O2−δ–Fe3−xCoxO4 (CGO-F(3−x)CxO) composites are one group of promising candidates. This study aims to understand the effect of the Fe/Co-ratio, i.e., x = 0, 1, 2, and 3 in Fe3−xCoxO4, on microstructure evolution and performance of the composite. The samples were prepared using the solid-state reactive sintering method (SSRS) to induce phase interactions, which determines the final composite microstructure. The Fe/Co ratio in the spinel structure was found to be a crucial factor in determining phase evolution, microstructure, and permeation of the material. Microstructure analysis showed that all iron-free composites had a dual-phase structure after sintering. In contrast, iron-containing composites formed additional phases with a spinel or garnet structure which likely contributed to electronic conductivity. The presence of both cations resulted in better performance than that of pure iron or cobalt oxides. This demonstrated that both types of cations were necessary to form a composite structure, which then allowed sufficient percolation of robust electronic and ionic conducting pathways. The maximum oxygen flux is jO2 = 0.16 and 0.11 mL/cm2·s at 1000 °C and 850 °C, respectively, of the 85CGO-FC2O composite, which is comparable oxygen permeation flux reported previously.

Abstract In this article, a versatile process based on microwave‐assisted sol–gel synthesis is introduced in order to apply a surface coating on cathode material for lithium‐ion batteries. Here, a nano‐scaled ZnO:Al (AZO) layer is coated homogeneously onto Li(Ni1/3Mn1/3Co1/3)O2 (NMC111) powder at temperatures below 210°C within a few minutes. In contrast to other wet‐chemical coating techniques, the method described here is conducted in a one‐pot reaction and does not require a post‐annealing step at elevated temperatures. Investigations via high resolution transmission electron microscopy (HR‐TEM), scanning transmission electron microscopy (STEM) and inductively‐coupled plasma optical emission spectroscopy (ICP‐OES) promote a thorough understanding of coating microstructure and quality in dependence of reaction temperature, duration and precursor concentration. The AZO protective coating on NMC111 significantly reduces capacity fading during cycling in the voltage range of 3.0‐4.5 V. Furthermore, applying optimal quantities of the coating agent on NMC111 lead to enhanced specific capacities compared to the uncoated material.

Asymmetric oxygen transport membranes have been extensively studied revealing the importance of the support porosity. In this study, asymmetric membranes with vertically channelled pores were prepared from Ba0.5Sr0.5(Co0.8Fe0.2)0.97Zr0.03O3-δ (BSCF-Z) by phase inversion tape casting. The rate-limiting effects of the membrane layer thickness, the support structure, and the activation layers were thoroughly analysed. This entails comparing the permeation rate of the samples with the membrane layer on different sides of the channelled supports. Pore tortuosity and computed permeability were evaluated from 3D-X-ray computed tomography and compared to previously reported asymmetric membranes prepared by tape-casting and freeze-drying. Due to a lower pore tortuosity, the channelled supports have an advantage in gas transport over the tape cast and freeze cast supports. However, this is compensated by a thicker membrane layer (∼54 μm) resulting in similar performance compared to the thinner membrane layers (∼20 μm) with freeze cast and tape cast supports.

Tungsten is foreseen presently as the plasma-facing material for divertors in fusion power plants. In order to achieve durable operation of divertors of current fusion reactors, an efficient way of maintaining the divertor functionality is needed. A system capable of in situ tungsten coating of the divertor via low-pressure plasma spraying was proposed to maintain the divertor integrity. In this work, tungsten was deposited on NB31 carbon fibre composite substrates using the low-pressure plasma spraying technology to evaluate the feasibility of this technique. The thickness, porosity, composition, adhesion, and microstructure of the coatings were investigated by scanning electron microscopy image analysis and energy dispersive spectroscopy. Based on the initial results, the spray parameters were iteratively improved in a campaign-based study. The coatings exhibited improving properties through an adjusting of the carrier gas flow, the scanning speed, and the spray distance. By lowering the carrier gas flow, the porosity of the coatings was reduced, resulting in coatings of 98% bulk density. Adjusting the carrier gas flow reduced the amount of semi-molten particles in the coatings significantly. A decrease in both scanning speed and spray distance increased the substrate’s temperature, which led to better adhesion and porosity.

Flash sintering, a special case of electric field-assisted sintering, results in accelerated densification at lower temperatures than conventional sintering methods. However, the mechanisms remain elusive despite the wide application potential. In-situ electron microscopy studies reveal shrinkage of ZnO green bodies due to both heating and heating/biasing but show no obvious effect of the current on the behavior. In contrast, thin epitaxial ZnO films deposited on an Al2O3 substrate undergo a clear flash event during in-situ voltage application in the TEM, providing the first observation of flash sintering of a thin film. The specimen was captured in the high conductivity state where grain boundary motion was observed. The microscopic origins of the high conductivity state could not be detected, but may have the same underlying physical origin as the high conductivity memristive state.

The aim of this work is to predict suitable chemical compositions for the development of new ceramic oxygen gas separation membranes, avoiding doping with toxic cobalt or expensive rare earths. For this purpose, we have chosen the system Sr1−xBax(Ti1−y−zVyFez)O3−δ (cubic perovskite-type phases). We have evaluated available experimental data, determined missing crystallographic information using bond-valence modeling and programmed a Python code to be able to generate training data sets for property predictions using machine learning. Indeed, suitable compositions of cubic perovskite-type phases can be predicted in this way, allowing for larger electronic conductivities of up to σe = 1.6 S/cm and oxygen conductivities of up to σi = 0.008 S/cm at T = 1173 K and an oxygen partial pressure pO2 = 10−15 bar, thus enabling practical applications.

Sodium is a promising candidate for stationary storage applications, especially when the demand for lithium-ion batteries increases due to electromobility applications. Even though its energy density is lower, Na-ion technology is estimated to lead to a cost reduction of 30% compared to Li-ion technology. To improve safety as well as energy density, Na-based all-solid-state-batteries featuring solid electrolytes such as beta-alumina and sodium superionic conductors and cathode materials such as Na3V2(PO4)3 and NaxCoO2 have been developed over the past years. However, the biggest challenge are mixed cathodes with highly conductive interfaces, especially when co-sintering the materials. For example, a promising sodium superionic conductor type Na3Zr2Si2PO12 electrolyte sinters at 1,250°C, whereas the corresponding Na3V2PO12 cathode decomposes at temperatures higher than 900°C, posing a bottleneck. Thus in this paper, we synthesized Na0.62 [Ni0.10Fe0.10Mn0.80]O2 as cathode material for all-solid-state sodium-ion batteries via a relatively cheap and easy solution-assisted solid state reaction processing route. The thermal investigations of the pure cathode material found no degradation up to 1,260°C, making it a perfect match for Na3.4Zr2Si2.4P0.6O12 electrolyte. In our aim to produce a co-sintered mixed cathode, electron microscopy investigation showed a highly dense microstructure and the elemental mapping performed via energy dispersive X-ray spectroscopy and secondary ion mass spectrometry confirm that Na3.4Zr2Si2.4P0.6O12 and Na0.62 [Ni0.10Fe0.10Mn0.80]O2 do not react during sintering. However, the active cathode material forms a sodium rich and a sodium deficient phase which needs further investigation to understand the origin and its impact on the electrochemical performance.

Three different ceramic matrix composites (CMCs) were produced using Cr2AlC as a matrix, and carbon, SiC and Al2O3 short fibers as a secondary phase. Cr2AlC powders were synthesized by solid-state reaction, followed by mixing with the fibers, and full densification using a field-assisted sintering technique. Of the three different fiber types, Carbon fibers reacted strongly with Cr2AlC, while the reaction with SiC fibers was more limited and alumina fibers didn’t show any reaction. Oxidation tests of the monolithic Cr2AlC and the composites were performed by thermogravimetric analysis. An alumina layer formed at 1000 ​°C on every sample, well attached and worked as a good oxidation barrier. Under realistic conditions using a burner rig for cyclic oxidation at 1200 ​°C for 500 cycles, the oxidation resistance of the alumina fiber CMC is good, as no defects or degradation are visible and the alumina layer is well attached.

Searching for next-generation electrocatalyst materials for electrochemical energy technologies is a time-consuming and expensive process, even if it is enabled by high-throughput experimentation and extensive first-principle calculations. In particular, the development of more active, selective and stable electrocatalysts for the CO2 reduction reaction remains tedious and challenging. Here, we introduce a material recommendation and screening framework, and demonstrate its capabilities for certain classes of electrocatalyst materials for low or high-temperature CO2 reduction. The framework utilizes high-level technical targets, advanced data extraction, and categorization paths, and it recommends the most viable materials identified using data analytics and property-matching algorithms. Results reveal relevant correlations that govern catalyst performance under low and high-temperature conditions.

Oxygen transport membranes can enable a wide range of efficient energy and industrial applications. One goal of development is to maximize the performance by the improvement of the material, microstructural properties and operational conditions. However, the complexity of the transportation processes taking place in such commonly asymmetric membranes impedes the identification of the parameters to improve them. In this work, we present a sensitivity study that allows identification of these parameters. It is based on a 1D transport model that includes surface exchange, ionic and electronic transport inside the dense membrane, as well as binary diffusion, Knudsen diffusion and viscous flux inside the porous support. A support limitation factor is defined and its dependency on the membrane conductivity is shown. For materials with very high ambipolar conductivity the transport is limited by the porous support (in particular the pore tortuosity), whereas for materials with low ambipolar conductivity the transport is limited by the dense membrane. Moreover, the influence of total pressure and related oxygen partial pressures in the gas phase at the membrane’s surfaces was revealed to be significant, which has been neglected so far in permeation test setups reported in the literature. In addition, the accuracy of each parameter’s experimental determination is discussed. The model is well-suited to guiding experimentalists in developing high-performance gas separation membranes.

Summary: Solid oxide fuel cells (SOFCs) exhibit potential to become a key technology for future clean energy systems. The metal-supported SOFC exhibits decisive strengths like fast start-up capability, mechanical robustness, and acceptable cost, making it the concept of choice for mobile applications. As a promising example, SOFC-powered range extenders for electric vehicles offer fast refueling and significantly increased driving range, while lowering size, weight, and the cost of the vehicle’s battery. Here, we report the development of a metal-supported SOFC aiming at exceptionally high power density. A knowledge-based improvement of all electrochemically active cell components enables a performance increase up to a factor of 10 and demonstrates the effectiveness of target-oriented optimization of processing and microstructure. Ultimately, enhanced cells meet the industrial performance target by providing a current density of 2.8 A × cm−2 at 650°C and 0.7 V, setting a benchmark for SOFC performance.

Metal exsolution is a dynamic process driven under a reducing atmosphere and at elevated temperatures that results in the self-assembly of nanoparticles at the surface of complex perovskite catalysts. The nanoparticle characteristics of metal exsolution catalysts can be subject to considerable inhomogeneity, and the anisotropic surface properties of ceramic oxides have been identified to have a major influence on the exsolution behavior. We systematically reveal the orientation-dependent anisotropy of the exsolution behavior of Ni in SrTi _0.9 Nb _0.05 Ni _0.05 O _3−δ using multi-faceted epitaxial thin films that represent a material system with properties in between functional ceramics and single-crystalline perovskite thin film model systems. Using an approach of combined orientation mapping and surface imaging we study the exsolution behavior with particular focus on the initial exsolution response, i.e. after short annealing times. We find orientation-specific variations in the surface morphology of the thin film facets. In the as-prepared state, surface reconstructions cause the formation of patterned surface structures for all thin film facets apart from (001) surfaces, which exhibit a plain surface morphology as well as an enhanced exsolution response. Surface reconstructions and their inherent energy landscape may hence cause an additional energy barrier for the exsolution reaction that results in orientation-dependent differences in the exsolution kinetics.

Tungsten (W) has the unique combination of excellent thermal properties, low sputter yield, low hydrogen retention, and acceptable activation. Therefore, W is presently the main candidate for the first wall and armor material for future fusion devices. However, its intrinsic brittleness and its embrittlement during operation bears the risk of a sudden and catastrophic component failure. As a countermeasure, tungsten fiber-reinforced tungsten (Wf/W) composites exhibiting extrinsic toughening are being developed. A possible Wf/W production route is chemical vapor deposition (CVD) by reducing WF6 with H2 on heated W fabrics. The challenge here is that the growing CVD-W can seal gaseous domains leading to strength reducing pores. In previous work, CVD models for Wf/W synthesis were developed with COMSOL Multiphysics and validated experimentally. In the present article, these models were applied to conduct a parameter study to optimize the coating uniformity, the relative density, the WF6 demand, and the process time. A low temperature and a low total pressure increase the process time, but in return lead to very uniform W layers at the micro and macro scales and thus to an optimized relative density of the Wf/W composite. High H2 and low WF6 gas flow rates lead to a slightly shorter process time and an improved coating uniformity as long as WF6 is not depleted, which can be avoided by applying the presented reactor model.

In the coming years, the demand for safe electrical energy storage devices with high energy density will increase drastically due to the electrification of the transportation sector and the need for stationary storage for renewable energies. Advanced battery concepts like all-solid-state batteries (ASBs) are considered one of the most promising candidates for future energy storage technologies. They offer several advantages over conventional Lithium-Ion Batteries (LIBs), especially with regard to stability, safety, and energy density. Hardly any recycling studies have been conducted, yet, but such examinations will play an important role when considering raw materials supply, sustainability of battery systems, CO2 footprint, and general strive towards a circular economy. Although different methods for recycling LIBs are already available, the transferability to ASBs is not straightforward due to differences in used materials and fabrication technologies, even if the chemistry does not change (e.g., Li-intercalation cathodes). Challenges in terms of the ceramic nature of the cell components and thus the necessity for specific recycling strategies are investigated here for the first time. As a major result, a recycling route based on inert shredding, a subsequent thermal treatment, and a sorting step is suggested, and transferring the extracted black mass to a dedicated hydrometallurgical recycling process is proposed. The hydrometallurgical approach is split into two scenarios differing in terms of solubility of the ASB-battery components. Hence, developing a full recycling concept is reached by this study, which will be experimentally examined in future research.

Because of an increasing interest in NaSICON materials as electrolyte materials in all-solid state sodium batteries, their thermal expansion was investigated in this study. The thermal expansion coefficient (CTE) of the Al and Y-substituted NaSICON compositions Na3+2xAlxYxZr2−2xSi2PO12 with 0 ≤ x ≤ 0.3 was obtained by dilatometry and compared to the CTE derived from the lattice parameters using high-temperature X-ray diffraction. The difference in CTE obtained from techniques, the influence of sodium content and central metal cation on CTE, as well as other observations such as phase changes are described and rationalized.

The retention of nanocrystallinity in dense ceramic materials is still a challenge, even with the application of external pressure during sintering. The compaction behavior of high purity and acetate enriched zinc oxide (ZnO) nano-powders was investigated. It was found that acetate in combination with water plays a key role during the compaction into green bodies at moderate temperatures. Application of constant pressure resulted in a homogeneous green body with superior packing density (86% of theoretical value) at moderate temperature (85 °C) in the presence of water. In contrast, no improvement in density could be achieved if pure ZnO powder was used. This compaction behavior offers superior packing of the particles, resulting in a high relative density of the consolidated compact with negligible coarsening. Dissolution accompanying creep diffusion based matter transport is suggested to strongly support reorientation of ZnO particles towards densities beyond the theoretical limit for packing of ideal monosized spheres. Finally, the sintering trajectory reveals that grain growth is retarded compared to conventional processing up to 90% of theoretical density. Moreover, nearly no radial shrinkage was observed after sinter-forging for bodies performed with this advanced processing method.

The gas flow through porous media including that of multiple species is frequently described by the binary friction model (BFM) considering the binary diffusion, Knudsen diffusion, and viscous flow. Therefore, a numerical simulation was performed on a microporous support of an asymmetric oxygen transport membrane. As its exact numerical solution is complicated and not always possible, the results of two different levels of simplification of the pressure profiles within the porous support are compared to the exact numerical solution. The simplification using a constant pressure equal to the gas pressure outside the support leads to a deviation by up to 0.45 mL·min−1·cm−2 from the exact solution under certain operating condition. A different simplification using a constant pressure averaged between the outside of the support and the support/membrane interface reduces this deviation to zero. Therefore, this is a useful measure to reduce computational efforts when implementing the Binary Friction Model in computational fluid dynamics simulations.